Recoil-induced ultrafast molecular rotation probed by dynamical rotational Doppler effect
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https://www.pnas.org/content/116/11/4877https://elib.sfu-kras.ru/handle/2311/128955
Автор:
Denis, Ceolina
Ji-Cai, Liu
Vinicius Vaz, Da Cruz
Hans, Agren
Loic, Journele
Renaud, Guillemin
Tatiana, Marchenko
Rajesh K. Kushawaha
Maria, Novella Piancastelli
Ralph, Puttnerf
Marc, Simon
Faris Gel’mukhanov
Коллективный автор:
Научно-исследовательская часть
Дата:
2019-03Журнал:
Proceedings of the National Academy of Sciences of the United States of AmericaКвартиль журнала в Scopus:
Q1Квартиль журнала в Web of Science:
Q1Библиографическое описание:
Denis, Ceolina. Recoil-induced ultrafast molecular rotation probed by dynamical rotational Doppler effect [Текст] / Ceolina Denis, Liu Ji-Cai, Da Cruz Vinicius Vaz, Agren Hans, Journele Loic, Guillemin Renaud, Marchenko Tatiana, Rajesh K. Kushawaha, Novella Piancastelli Maria, Puttnerf Ralph, Simon Marc, Faris Gel’mukhanov // Proceedings of the National Academy of Sciences of the United States of America. — 2019. — Т. 116 (№ 11). — С. 4877-4882Текст статьи не публикуется в открытом доступе в соответствии с политикой журнала.
Аннотация:
Observing and controlling molecular motion and in particular rotation are fundamental topics in physics and chemistry. To initiate ultrafast rotation, one needs a way to transfer a large angular momentum to the molecule. As a showcase, this was performed by hard X-ray C1s ionization of carbon monoxide accompanied by spinning up the molecule via the recoil “kick” of the emitted fast photoelectron. To visualize this molecular motion, we use the dynamical rotational Doppler effect and an X-ray “pump-probe” device offered by nature itself: the recoil-induced ultrafast rotation is probed by subsequent Auger electron emission. The time information in our experiment originates from the natural delay between the C1s photoionization initiating the rotation and the ejection of the Auger electron. From a more general point of view, time-resolved measurements can be performed in two ways: either to vary the “delay” time as in conventional time-resolved pump-probe spectroscopy and use the dynamics given by the system, or to keep constant delay time and manipulate the dynamics. Since in our experiment we cannot change the delay time given by the core-hole lifetime τ, we use the second option and control the rotational speed by changing the kinetic energy of the photoelectron. The recoil-induced rotational dynamics controlled in such a way is observed as a photon energy-dependent asymmetry of the Auger line shape, in full agreement with theory. This asymmetry is explained by a significant change of the molecular orientation during the core-hole lifetime, which is comparable with the rotational period.
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